ConspectusAs the world transitions away from fossil energy to green and renewable energy, electrochemical energy storage increasingly becomes a vital component of the mix to conduct this transition. The central goal in developing next-generation batteries is to maximize the gravimetric and volumetric energy density and battery cycle life and improve safety. All solid-state batteries using a solid electrolyte and a lithium metal anode represent one of the most promising technologies that can achieve this goal. Highly conductive solid electrolytes (>10 mS·cm-1) are the key component to remove the safety concerns inherent with flammable organic liquid electrolytes and achieve high energy density by enabling high active material loading. Considering a range of inorganic solid electrolytes that have been developed to date, sulfide solid electrolytes exhibit the highest ionic conductivities, which even surpass those of conventional organic liquid electrolytes. Argyrodite-structured sulfide solid electrolytes are among the most promising materials in this class and are currently the dominantly used solid electrolytes for all-solid-state battery fabrication. Argyrodite solid electrolytes are particularly appealing because of their ultrahigh Li-ion conductivity, quasi-stable solid-electrolyte interphase (SEI) formed with Li metal, and ability to be prepared via scalable solution-assisted synthesis approaches. These factors are all vital for commercial applications.In this Account, we afford an overview of our recent development of several argyrodite superionic conductors, including Li6.6Si0.6Sb0.5S5I (24 mS·cm-1), Li6.6Ge0.6P0.4S5I (18 mS·cm-1), and Li5.5PS4.5Cl1.5 (12 mS·cm-1), and a comprehensive understanding of the origin of the underlying high conductivity, namely, sulfide/halide anion site disorder and Li cation site disorder. A high degree of sulfide/halide anion site disorder (changes in anion distribution) modifies the anionic charge, which in turn strongly influences the lithium distribution. A more inhomogeneous charge distribution in anion-disordered systems generates a spatially diffuse and delocalized lithium density, resulting in faster ionic transport. Lithium cation site disorder generated by increasing Li carrier concentration through aliovalent substitution creates high-energy interstitial sites for Li ion diffusion, which activate concerted ion migration and flatten the energy landscape for Li ion diffusion. This enables high conductivity in Li-rich argyrodite superionic conductors. These concepts are also expected to promote the design of rational new solid electrolytes and fundamental understanding of the structure-ion transport relationships in inorganic ionic conductors.Collectively, a comprehensive and deep understanding of the interphase formation between argyrodite solid electrolytes and cathode active materials/Li metal and the failure mechanism of all-solid-state batteries with argyrodite solid electrolytes will lead to the bottom-up engineering of the cathode/anode-solid electrolyte interfaces, which will accelerate the development of safe, high-energy-density all-solid-state lithium batteries.

Innovative Approaches to Li-Argyrodite Solid Electrolytes for All-Solid-State Lithium Batteries.

The effect of hole localization on photocatalytic activity of Pt-tipped semiconductor nanocrystals is investigated. By tuning the energy balance at the semiconductor-ligand interface, we demonstrate that hydrogen production on Pt sites is efficient only when electron-donating molecules are used for stabilizing semiconductor surfaces. These surfactants play an important role in enabling an efficient and stable reduction of water by heterostructured nanocrystals as they fill vacancies in the valence band of the semiconductor domain, preventing its degradation. In particular, we show that the energy of oxidizing holes can be efficiently transferred to a ligand moiety, leaving the semiconductor domain intact. This allows reusing the inorganic portion of the \"degraded\" nanocrystal-ligand system simply by recharging these nanoparticles with fresh ligands.

/pdf/the-role-of-hole-localization-in-sacrificial-hydrogen-16ccznihzx.pdf

The Role of Hole Localization in Sacrificial Hydrogen Production by Semiconductor-Metal Heterostructured Nanocrystals

Exosomes are cell-derived structures packaged with lipids, proteins, and nucleic acids. They exist in diverse bodily fluids and are involved in physiological and pathological processes. Although th...

Label-Free Isolation of Exosomes Using Microfluidic Technologies.

Sedimentation field-flow fractionation

Hyperlayer field-flow fractionation is proposed as a method designed to overcome some of the limitations of conventional field-flow fractionation (FFF). In hyperlayer FFF, steady-state particle layers are formed above the channel wall by the combination of a primary field (e.g., sedimentation or electrical) and a secondary gradient (such as density of pH). Such zones could be separated along the flow axis in FFF even if they strongly overlap in the field or lateral direction. An approximate theory is derived for sedimentation hyperlayer FFF, showing both the rate of zone migration and the extent of peak broadening. Calculations are presented which show that the system should be highly effective for the separation of particles in the vicinity of μm in diameter or larger.

Hyperlayer field-flow fractionation

Mesoporous silica nanoparticles (MSN) with enlarged pores were prepared and characterized, and reversibly dissociated subunits of concanavalin A were entrapped in the mesopores, as shown by multiple biochemical and material characterizations. When loaded in the MSN, we demonstrated protein stability from proteases and, upon release, the subunits reassociated into active proteins shown through mannose binding and o-phthalaldehyde fluorescence. We have demonstrated a versatile and facile method to load homomeric proteins into MSN with potential applications in enhancing the delivery of large therapeutic proteins.

Conserved Activity of Reassociated Homotetrameric Protein Subunits Released from Mesoporous Silica Nanoparticles.

Asymmetrical Flow Field Flow Fractionation for Molar Mass Characterization of Polyethylene Oxide in Abuse-Deterrent Formulations.

Lithium sulfide (Li2S) is a key component and major cost driver for sulfide-based solid-state electrolytes. However, this material is not commercially available in nanocrystal form. We previously demonstrated solution-based synthesis of Li2S nanocrystals (NCs) with tunable size in a small Parr reactor and validated their potential as cathode active materials. Herein, we report on the scale-up of both the synthesis and purification steps, generating meaningful quantities for solid-state electrolyte formation. Use of a bubble column reactor significantly increased production capacity by two orders of magnitude, from~100 mg/batch to >10 g/batch. An evaporator/condenser and fluidized bed with corresponding capacity were introduced for solvent evaporation and annealing, respectively. Intrinsic purity, thermal stability, and morphology of those NCs are characterized by XRD, TGA, and SEM respectively. It is shown that the NC size and purity could be tuned by varying the annealing temperature. Li2S-P2S5 based glassy electrolytes formed by a combination of ball milling and cold pressing were used to illustrate the benefits of these Li2S NCs. It was shown that Li2S NCs reduced the mechanical ball mixing time required to make Li2S-P2S5 based glasses by at least 70% relative to commercial Li2S micro-powders. 70Li2S-30P2S5 glassy electrolytes were fabricated by cold pressing at various pressures and characterized by impedance spectroscopy and chronoamperometry. SSEs formed at the optimum condition exhibited high ionic conductivity (~10−5 s cm−1), low electronic conductivity (~10−10 s cm−1), and reasonable activation barrier (~35 kJ mol−1). These properties were comparable to leading reports in the literature, validating the use of our material for solid-state electrolyte fabrication.

https://iopscience.iop.org/article/10.1149/1945-7111/ab6e3f/pdf

Scalable Synthesis of Li2S Nanocrystals for Solid-State Electrolyte Applications

Field-flow fractionation (FFF) is an increasingly important family of techniques for macromolecular separations spanning synthetic, biological, and natural polymers and intricate complexes. FFF's many advantageous characteristics originate from its open channel (no packing material) and the ability to relate retention time to physicochemical properties of the analyte using FFF theory. Normal mode separation of analytes up to ~ 1 μm in size in a single channel provides a wide applicable size range. When FFF is coupled with online concentration and light scattering detectors, detailed information about molecular weight, size, and conformation distributions may be obtained. Flow and thermal FFF are the two main techniques for polymer analyses and are the subjects of this chapter. Asymmetrical flow FFF separates by differences in diffusion coefficient while thermal FFF is sensitive to (co)polymer composition and polymer architecture. This chapter first introduces readers to FFF fundamentals and then gives detailed descriptions of flow and thermal FFF theory, experimentation, and applications.

Field-flow fractionation techniques for polymer characterization

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Conserved Activity of Reassociated Homotetrameric Protein Subunits Released from Mesoporous Silica Nanoparticles.

Asymmetrical Flow Field Flow Fractionation for Molar Mass Characterization of Polyethylene Oxide in Abuse-Deterrent Formulations.

Scalable Synthesis of Li2S Nanocrystals for Solid-State Electrolyte Applications

Field-flow fractionation techniques for polymer characterization